CC BY 4.0 UnportedSabaghi, DavoodWang, ZhiyongBhauriyal, PreetiLu, QiongqiongMorag, AhiudMikhailovia, DariaHashemi, PayamLi, DongqiNeumann, ChristofLiao, ZhongquanDominic, Anna MariaNia, Ali ShayganDong, RenhaoZschech, EhrenfriedTurchanin, AndreyHeine, ThomasYu, MinghaoFeng, Xinliang2023-06-022023-06-022023https://oa.tib.eu/renate/handle/123456789/12274http://dx.doi.org/10.34657/11306The anion-intercalation chemistries of graphite have the potential to construct batteries with promising energy and power breakthroughs. Here, we report the use of an ultrathin, positively charged two-dimensional poly(pyridinium salt) membrane (C2DP) as the graphite electrode skin to overcome the critical durability problem. Large-area C2DP enables the conformal coating on the graphite electrode, remarkably alleviating the electrolyte. Meanwhile, the dense face-on oriented single crystals with ultrathin thickness and cationic backbones allow C2DP with high anion-transport capability and selectivity. Such desirable anion-transport properties of C2DP prevent the cation/solvent co-intercalation into the graphite electrode and suppress the consequent structure collapse. An impressive PF6−-intercalation durability is demonstrated for the C2DP-covered graphite electrode, with capacity retention of 92.8% after 1000 cycles at 1 C and Coulombic efficiencies of > 99%. The feasibility of constructing artificial ion-regulating electrode skins with precisely customized two-dimensional polymers offers viable means to promote problematic battery chemistries.enghttps://creativecommons.org/licenses/by/4.0500aniondurabilityelectrodefuel cellgraphitemembraneArticle